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Engineering a dual?single?atom catalyst with an aptamer?defined confined reactive milieu mimics enzymatic precision. This architecture orchestrates spatiotemporal control by synchronizing radical generation with substrate pre?enrichment, achieving >87% selectivity while slashing non?specific mineralization to 90% mineralization), establishing a universal strategy for decoupling intrinsic activity from selectivity in complex chemical environments.ABSTRACTSpatiotemporal control of short?lived reactive intermediates remains a central challenge in heterogeneous catalysis, as non?selective diffusion fundamentally limits efficiency in complex media. Inspired by enzymatic compartmentalization, we report an aptamer?functionalized Au?Fe dual?single?atom catalyst (Apt?Au1?Fe1/NC) that mimics nature's precision by integrating atomically dispersed Au?Fe sites with a genetically engineered recognition element. This material design creates a “smart reactive pocket” featuring two synergistic interfaces: the Au?Fe heteronuclear pair electronically modulates the d?band center to lock the oxygen reduction reaction (ORR) into a highly selective 3?electron pathway with a lowered energy barrier (0.424 eV), while the grafted aptamer acts as a molecular gatekeeper for substrate pre?enrichment. The resulting architecture achieves exceptional selectivity (87.0%–92.6%) for specific targets while suppressing non?specific mineralization to below 5.3%—a stark contrast to conventional systems where selectivity is negligible and mineralization exceeds 90%. Mechanistically, the synergistic electronic interaction ensures localized ·OH generation, while the aptamer enforces a strict “proximity effect,” confining these radicals within the nanoscale space for instantaneous consumption by captured substrates. By imposing biological recognition?based spatial constraints on inorganic active centers, this work establishes a universal paradigm for decoupling activity from selectivity, enabling precision chemical conversion in complex matrices.